2018 2D Layered Material Based Van Der Waals Heterostructures For Optoelectronics PDF

FEATURE ARTICLE
2D Materials www.afm-journal.de
2D Layered Material-Based van der Waals Heterostructures

for Optoelectronics
Xing Zhou, Xiaozong Hu, Jing Yu, Shiyuan Liu, Zhaowei Shu, Qi Zhang, Huiqiao Li,
Ying Ma, Hua Xu,* and Tianyou Zhai*
1. Introduction
Van der Waals heterostructures (vdWHs) based on 2D layered materials
with selectable materials properties pave the way to integration at the Graphene has ignited intensive attention
atomic scale, which may give rise to fresh heterostructures exhibiting since it was mechanically exfoliated in
absolutely novel physics and versatility. This feature article reviews the 2004[1] due to the high carrier mobility,[1,2]
state-of-the-art research activities that focus on the 2D vdWHs and their ultralarge specific surface area,[3] high
in-plane thermal conductivity and rela-
optoelectronic applications. First, the preparation methods such as tively low out-of-plane value,[4–7] and
mechanical transfer and chemical vapor deposition growth are comprehen- relatively low Young’s modulus[8] which
sively outlined. Then, unique energy band alignments generated in inspire a wide range of promising appli-
2D vdWHs are introduced. Furthermore, this feature article focuses on the cations such as ultrafast high-frequency
applications in light-emitting diodes, photodetectors, and optical modula- photodetectors,[9–11] transparent conduc-
tive electrodes,[12] and broadband optical
tors based on 2D vdWHs with novel constructions and mechanisms. The
modulators.[13] However, the research of
recently reported novel constructions of the devices are introduced in three graphene has been severely hampered
primary aspects: light-emitting diodes (such as single defect light-emitting due to the absence of a bandgap, which
diodes, circularly polarized light emission arising from valley polarization), results in a small current on/off ratio for
photodetectors (such as photo-thermionic, tunneling, electrolyte-gated, graphene transistors.[14] Thus, other 2D
and broadband photodetectors), and optical modulators (such as graphene layered materials (2DLMs) with varying
bandgaps[15] including semimetals (such
integrated with silicon technology and graphene/hexagonal boron nitride as WTe2[16–18]), topological insulators (such
(hBN) heterostructure), which show promising applications in the next- as Pb1−xSnxTe,[19] Bi2Te3[20,21]), semiconduc-
generation optoelectronics. Finally, the article provides some conclusions tors (such as black phosphorous (BP),[22–24]
and an outlook on the future development in the field. MoS2,[25–31] WS2,[32–36] WSe2[37,38]), insula-
tors (such as boron nitride (BN)[39–42]). Dif-
ferent from gapless graphene, these 2DLMs
possess bandgaps in a wide range and can
also be modulated with the changing thickness, which have trig-
Dr. X. Zhou, X. Z. Hu, J. Yu, Z. W. Shu, Dr. Q. Zhang, Prof. H. Q. Li,
Prof. Y. Ma, Prof. T. Y. Zhai
gered tremendous interest in many fields such as field effect
State Key Laboratory of Material Processing transistors,[30,43–46] photodetectors,[47–53] flexible devices.[54–58]
and Die & Mould Technology van der Waals heterostructures (vdWHs) based on these
School of Materials Science and Engineering 2DLMs with selectable materials properties pave the way to
Huazhong University of Science and Technology (HUST) integration at the atomic scale which may give rise to fresh
Wuhan 430074, P. R. China
E-mail: zhaity@hust.edu.cn heterostructures exhibiting absolutely novel physics and versa-
Prof. S. Liu tility.[59–62] Generally, these 2DLM-based vdWHs could be real-
State Key Laboratory of Digital Manufacturing Equipment ized by mechanical transfer or chemical vapor deposition (CVD)
and Technology growth.[63–65] Compared with the conventional semiconductor-
Huazhong University of Science and Technology (HUST) based heterostructures which require the severely similar lattice
Wuhan 430074, P. R. China
structures of the component semiconductors, vdWHs can release
Prof. H. Xu
Key Laboratory of Applied Surface and Colloid Chemistry
the strict lattice mismatching requirement due to the weak inter-
Ministry of Education action between the adjacent layers.[66,67] Furthermore, the inter-
School of Materials Science and Engineering face can be atomically sharp and the thickness can be as thin
Shaanxi Normal University as a few atomic layers, and the stacking sequence can be artifi-
Xi’an 710119, P. R. China cially arranged to obtain novel physical properties. Thus, as the
E-mail: xuhua-nano@snnu.edu.cn
extending field of 2D materials, vdWHs has been growing fast.
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/adfm.201706587.
Herein, we review the recent progress of 2D vdWHs,
and mainly focus on the preparation methods, energy band
DOI: 10.1002/adfm.201706587 alignments of two or more stacked 2DLMs, and the optoelectronic
Adv. Funct. Mater. 2018, 1706587 1706587 (1 of 28) © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com www.afm-journal.de
applications. First, we summarize the preparation methods of

vdWHs including mechanical transfer and CVD growth. Then, Xing Zhou received his
the novel energy band alignments of vdWHs are discussed B.S. degree in inorganic non-
including the interlayer coupling and the exciton dynamics of metallic materials from the
interlayer transition. The optoelectronic applications are dis- Wuhan University of Science
cussed in detail for the 2D vdWHs-based light-emitting diodes and Technology (WUST) in
(LEDs), photodetectors, and optical modulators with different 2012, and then received his
constructions. Finally, the conclusions and outlook of 2D vdWHs Ph.D. degree in Materials
are presented. from the School of Materials
Science and Engineering,
Huazhong University of
Science and Technology
2. Preparation Methods of vdWHs
(HUST) in 2017. Currently,
Up to now, reliable preparation methods of 2D vdWHs are of he is an assistant professor
great significance for further investigation and applications. in the School of Materials Science and Engineering at the
Mechanical transfer[68–72] and CVD growth[63,65,73] are the most HUST. His research concentrates on the controllable syn-
used methods for preparing 2D vdWHs. In the following con- thesis of 2D group IV–VI semiconductors and heterostruc-
text, we will focus on these two methods. tures via CVD methods for electronic and optoelectronic
applications.
2.1. Mechanical Transfer Hua Xu received his

B.S. degree in chemistry
Mechanical transfer is one of the most commonly used methods from the Ningxia University
to fabricate the 2D vdWHs once the few-layer or monolayer mate- in 2007, and then received
rials were prepared by mechanical exfoliation from their bulk his Ph.D. degree in organic
counterparts or CVD growth. Generally, it is easy to construct the chemistry from the Lanzhou
different stacking orders of 2D vdWHs artificially as shown in University under the joint
Figure 1a. First, the atomic layers prepared by mechanical exfo- supervision of Prof. Haoli
liation or CVD growth are transferred onto the targeted substrate Zhang and Prof. Jin Zhang
(such as SiO2/Si). Next, the second atomic layer can be either (Peking University) in 2012.
dry exfoliated or wet transferred on a sacrificial polymer such He then worked as an
as poly(methyl methacrylate) (PMMA). Then, the atomic layer Associate Professor at the
with the PMMA is transferred onto a transparent stamp such School of Materials Science and Engineering, Shaanxi
as poly(dimethylsiloxane) (PDMS), and is located on the desired Normal University (SNNU). His research interest is
position employing the micromanipulators under the objective focused on the design, synthesis, and characterization of
lens, and lowered down until the two atomic layers contacting to 2D nanomaterials for promising applications in electronic,
form vdWH. Then, the polymers can be directly dissolved in sol- optoelectronic, and new energy devices.
vents.[74] However, the dissolved polymers will leave the residue
on the surface of 2D materials, hindering further stacking. Thus, Tianyou Zhai received his
to realize the complex multilayer stacking artificially without res- B.S. degree in chemistry from
idue between the individual layers, more strategies such as pick- the Zhengzhou University
up have been reported.[75] First, a silicon substrate is coated with in 2003, and then received
poly(propylene carbonate) (PPC), and one kind of target crystals his Ph.D. degree in physical
is mechanically exfoliated onto the PPC film. Then, the PPC film chemistry from the Institute
is transferred onto a piece of PDMS with the exfoliated flake-side of Chemistry, Chinese
up. The PDMS is then fixed to a glass slide. On the other hand, Academy of Sciences (ICCAS)
flakes of other target materials are exfoliated on different silicon in 2008. Afterward, he joined
substrates. Then, the vdWHs can be realized by picking up dif- the National Institute for
ferent layers one by one assisted by the PPC film without residue Materials Science (NIMS) as
left between the individual layers. The glass slide and PDMS can a JSPS postdoctoral fellow,
be separated from the vdWH with PPC after heating to 90 °C via and then as an ICYS-MANA researcher within the NIMS.
softening the PPC,[75] with the 2D vdWH left on the substrate. Currently, he is a Chief Professor of School of Materials
Finally, the PPC or PMMA can be removed in chloroform or Science and Engineering, Huazhong University of Science
acetone, leaving the 2D vdWHs on the substrate. The advanced and Technology (HUST). His research interests include
pick-up method results in clean interfaces and allows the stacking the controlled synthesis and exploration of fundamental
orders or crystal orientation of these 2DLMs to be adjusted artifi- physical properties of inorganic functional nanomaterials,
cially which may result in novel physical properties. For example, as well as their promising applications in energy science,
a vdWH based on monolayer MoS2 and WSe2 is demonstrated in electronics, and optoelectronics.
Figure 1b, and the electron diffraction pattern of the hetero-bilayer
Figure 1. a) Schematic illustration of the transfer process for 2D vdWHs. b) Optical microscope image of a WSe2/MoS2 hetero-bilayer on a Si/SiO2
substrate (260 nm SiO2). c) High resolution transmission electron microscopy (HRTEM) images of a boundary region of monolayer MoS2 and the
hetero-bilayer, showing the resulting Moiré pattern. d) The electron diffraction pattern of the hetero-bilayer shown in (b), with the pattern of MoS2
and WSe2 indexed in green and blue colors, respectively. (b–d) Reproduced with permission.[76] Copyright 2014, National Academy of Sciences of the
United States of America. e) High-resolution Scanning transmission electron microscopy (STEM) image of the same heterostructure, consisting of
four layers of MoS2 and WSe2. Right: Electron dispersion X-ray spectroscopy (EDS) mapping of the heterostructure. Reproduced with permission.[133]
Copyright 2015, American Chemical Society.
WSe2/MoS2 along the [001] zone axis in Figure 1c demonstrates MoSe2. Xu and co-workers[65] employed the mixture of WSe2
that in this specific hetero-bilayer structure, the two hexagonal and MoSe2 powder as sources and obtained MoSe2/WSe2 lat-
reciprocal lattices are rotated by 12.5° with respect to each layer eral heterostructures at a growth temperature of 950 °C with
without obvious lattice strain, resulting in moiré fringes with a the system pressure maintained at ≈7 Torr. Then, Duan et al.[85]
spatial periodicity on the order of four to six times the lattice con- synthesized WS2/WSe2 lateral heterostructures through evap-
stants of each layer.[76] The atomically sharp interface of the het- orating WS2 at 1057 °C and followed by evaporating WSe2
erostructure can be obtained by this stacking process confirmed at 1190 °C while under ambient pressure. However, these
by the high-resolution cross-sectional scanning transmission elec- methods via evaporating the source materials usually need
tron microscope image of the heterostructure (Figure 1d). Fur- much high temperatures, which may make the reaction condi-
thermore, the complex 2D vdWHs with more stacking layers can tions uncontrollable. Ajayan and co-workers[73] used S, W, MoO3
be realized by this mechanical transfer process. powders as S, W, Mo precursors, respectively, and with the
Mechanical transfer process provides a lot of flexibility in addition of Te powder to accelerate the melting of W powder
constructing diverse 2D vdWHs with various materials which during the growth as shown in Figure 2a, thus the growth tem-
may give rise to fresh physical properties, it is not scalable, perature was decreased. Furthermore, the precise temperature
which is imperative for further practical applications in elec- and the different nucleation and growth rates determine the
tronics and optoelectronics. Alternatively, the bottom-up final products: vertical heterostructures dominate at ≈850 °C
method such as direct CVD synthesis of 2D vdWHs has been (Figure 2b,c), while lateral heterostructures are preferred at
successful in synthesizing graphene- or transition metal dichal- ≈650 °C (Figure 2d,e). These different heterostructures modu-
cogenide (TMD)-based vdWHs,[77–79] which shows promising lated by temperatures mainly are related with the nucleation
applications in scalable production. and growth rate of each layer. At low temperatures (650 °C),
nucleation and growth of WS2 are extremely difficult and slow.
Attaching WS2 to the MoS2 edge with strong chemical bonding,
2.2. CVD Growth however, results in much smaller nucleation energy than on
the surface of MoS2, which leads to in-plane heterostructure, a
CVD growth has shown booming development in the last dec- kinetic product preferred at low temperatures. At high tempera-
ades such as the CVD growth of graphene[80,81] and TMDs,[82,83] tures (850 °C), the environment would provide enough energy
and has been employed for synthesizing 2D vdWHs recently.[84] to overcome the nucleation barrier. In this case, the kinetic
The most used method for CVD growth of 2D vdWHs is that effect would not be critical and the thermodynamically more
evaporating the target sources such as WS2, WSe2, MoS2, stable product becomes preferable. Thus, the WS2/MoS2 bilayer
Figure 2. a) Schematic diagram of the synthesis for heterostructures. b,c) Schematic, optical images of the vertically stacked WS2/MoS2 heterostructure.
d,e) Schematic, optical images of the WS2/MoS2 in-plane heterostructure. f) PL spectra taken from the four points marked in (c). g) Z-contrast image
of the step edge of the WS2/MoS2 bilayer. The green dashed line indicates the step edge, and the two triangles indicate the orientation of the MoS2
(top part of image) and WS2 (bottom part) layers. Inset: Fast Fourier transform of the Z-contrast image showing only one set of diffraction patterns.
Reproduced with permission.[73] Copyright 2014, Nature Publishing Group.
heterostructure is preferred at higher temperatures. These graphene- and TMD-based 2D vdWHs realized by two-step CVD
different structures induce novel physical properties in the growth.[77,79,86–94] Li and co-workers[63] realized the lateral WSe2/
2D vdWHs as shown in Figure 2f. The photoluminescence (PL) MoS2 heterostructure with high quality and sharp interface,
spectra acquired from the monolayer region (points 1 and 2 where WSe2 is grown on substrates through vdW epitaxy fol-
in Figure 2c) exhibit a strong peak at the wavelength of 680 nm, lowed by the edge epitaxial growth of MoS2 along the W growth
indicating the 1.82 eV direct excitonic transition energy in front as shown in Figure 3a. Two-step growth promises precise
monolayer MoS2, while three main peaks are observed at wave- control to the atomically sharp interface. The as-synthesized
lengths of 630, 680, and 875 nm, respectively (points 3 and 4). WSe2/MoS2 lateral heterostructures are clearly observed from
The peaks at 630 nm (1.97 eV) and 680 nm (1.82 eV) are attrib- the optical image in Figure 3b, showing the clear domain and
uted to the direct excitonic transition energies in WS2 and MoS2. uniformity. Besides, the atomically sharp interface between the
The comparable intensity of the peak at 875 nm to that of its WSe2 and MoS2 is observed in Figure 3c. Furthermore, Zhai and
individual monolayer components observed in the bilayer co-workers[95] synthesized SnSe2/MoS2 vertical heterostructures
sample indicates a possible direct excitonic transition at this using monolayer MoS2 triangles as templates, with the top SnSe2
energy range, which suggests that the coupling between WS2 nearly covering the bottom MoS2 as shown in Figure 3d. As dem-
and MoS2 results in the unprecedented direct bandgap with onstrated in Figure 3e, the atomic-resolution Z-contrast image
reduced energy. Figure 2g shows the atomic-resolution Z-con- from the edge of the heterostructure shows the top SnSe2 and
trast image from a step edge of the vertical heterojunction. bottom MoS2 with highly symmetric crystallographic directions
The alternative bright and dark atomic column arrangement in matching well with the atomic models in the inset of Figure 3e,
the hexagonal lattice indicates that the as-synthesized vertical which indicates the 2H phase of both SnSe2 and MoS2. Then,
WS2/MoS2 heterostructure presents the 2H stacking, where the the Raman spectroscopy is employed to evaluate the crystal struc-
bright W and dark Mo atoms are aligned with S2, respectively. tures and vibrational properties as shown in Figure 3f. The main
However, the W and Mo substitutions can be found in the other peaks of SnSe2 (Eg ≈ 110 cm−1, A1g ≈ 185 cm−1) and MoS2 (E2g1 ≈
side occasionally with this one-step CVD growth, means the big 385 cm−1, A1g ≈ 405 cm−1) are all observed. However, the Eg peak
discount of the sharp interface. Thus, there are several attempts of SnSe2 shows absolutely redshift of 6 cm−1 (may be induced
on two-step CVD growth of 2D vdWHs which may protect the by the built-in strain resulting from the large lattice mismatch of
atomically sharp interface at the junction. The most studied are these two components), whereas the A1g peak shifts only 1 cm−1
Figure 3. a) Schematic illustration of the sequential growth of the monolayer WSe2–MoS2 in-plane heterostructure. b) Optical image of the WSe2–MoS2
heterostructure. c) High-resolution STEM image taken from the WSe2–MoS2 in-plane heterostructure. (a–c) Reproduced with permission.[63] Copyright
2015, American Association for the Advancement of Science. d) Schematic of SnSe2/MoS2 heterostructures by epitaxial growth. e) An atomic-resolution
Z-contrast image from the edge of the triangle. f) Raman spectra of single SnSe2, MoS2, and the SnSe2/MoS2 heterostructure. (d–f) Reproduced with
permission.[95] Copyright 2017, Institute of Physics. g) Scanning electron microscopy (SEM) image of epitaxial PbS nanoplates heterostructure on
graphene/SiO2/Si substrate. The right image shows that the PbS nanoplates grows along edge of graphene ribbon with <110> orientation as shown
in the inset. (g) Reproduced with permission.[102] Copyright 2016, John Wiley & Sons, Inc. h,i) Schematic, optical image of the PbS nanoplates–MoS2
heterostructures. j) Schematic image of edge contact between the MoS2 and PbS. Inset is a top view of the schematic. Reproduced with permission.[103]
(may be induced by the strong electron–phonon coupling at the the edge area results from the abundant unsaturated Mo atoms
interface of the junction). These reported graphene- and TMD- along the edge of MoS2, which increase the possibility that the
based heterostructures are limited to those materials with sim- PbS nanoplates are primarily nucleated at the edge.
ilar superlattices, thus it is still in great challenge to synthesize As mentioned above, the construction of vdWHs via mechan-
a variety of different vdWHs, especially for those possessing ical transfer process is not limited by conventional lattice-matching
incommensurate superlattices, which may lead to unique band constraints. Thus, it provides a great deal of flexibility in fabri-
alignments or structures. For example, many nonlayered mate- cating various kinds of vdWHs integrated with diverse materials
rials such as CdSe,[96] CdTe,[97] PbS[98–100] exhibit excellent opto- artificially, which may induce disparate properties. However,
electronic properties. Thus, combination of such nonlayered the thickness and size of the vdWHs fabricated by mechanical
materials with layered materials may construct a new type of transfer process are usually uncontrollable, and the efficiency of
2D vdWHs to offer fresh platform for applications in electronics constructing vdWHs fabricated by mechanical transfer process
and optoelectronics.[101–103] Hu and co-workers[101] synthesized is too low. Besides, residues at the interface of the vdWHs fabri-
CdS/MoS2 2D vdWHs through epitaxial growth with the CdS cated by mechanical transfer process are usually unavoidable,
nanoplates distributed on the MoS2 triangles uniformly. Fur- which may impede the properties of the vdWHs. Thus, it is not
thermore, He and co-workers[102,103] fabricated nonlayered PbS– suitable and scalable for industrial integration. In contrast, CVD
graphene (Figure 3g) and PbS–MoS2 heterostructures with edge growth[104,105] has been proposed as an alternative way to synthe-
contacts along the [110] direction (Figure 3h,i). As shown in size single-crystalline 2D semiconductors, due to the advantages
Figure 3j, the Mo atoms of the zigzag edge of MoS2 are bonded over the precise control on morphology, defects, and structure of
with the S atoms chain exposed to PbS (110). A high activity of final products, particularly on large-area growth of 2D materials
such as graphene,[80,81] TMDs.[82,83] Also, it has been employed for and affect the electronic band structures in each layer.[111–177]
synthesizing 2D vdWHs recently.[84] The size, morphology, and The interlayer coupling between two vdW-stacked 2D layers
thickness can be precisely adjusted by the gas flux, mass of precur- can be modulated from noninteraction to strong interaction,
sors, temperature of reaction, substrate, and so on.[106–110] Thus, resulting in novel physical properties.
CVD growth is highly promising for fabricating vdWHs in large- Graphene has ultrahigh carrier mobility (≈104 cm2 V−1 s−1)[1]
scale. Whereas, CVD growth is usually limited by highly sensitive due to the linear dispersion of the Dirac electrons. However,
growth conditions for each 2DLM, which makes it difficult to mix the applications in transistors have been impeded by the zero
and match high-quality atomic layers without damaging the inter- bandgap of graphene.[49,178] Thus, the vdWHs based on gra-
face such as the atom diffusion. Thus, CVD growth of vdWHs phene have leaded many booming research fields, which may
is still at the initial stage and remains a great challenge for the make up for the shortage of the zero bandgap of graphene.
industrial integration. For example, random rotational orientation between the gra-
phene and hBN lattices will be induced when constructing gra-
phene on hBN devices. This rotation between the lattices and
3. Energy Band Alignments of vdWHs the longer lattice constant of hBN result in topographic moiré
patterns as shown in Figure 4a–c.[179] This moiré pattern acts
The vdW interactions between the adjacent layers at the inter- as a weak periodic potential and thereby results in the emer-
face are weak, while their electron orbitals extend to each other gence of a new set of Dirac points in Figure 4d.[179] This result
Figure 4. a–c) Scanning tunneling microscopy (STM) topography images showing 2.4 nm (a), 6.0 nm (b), and 11.5 nm (c). d) Experimental dI = dV curves
for two different moiré wavelengths, 9.0 nm (black) and 13.4 nm (red). The dips in the dI = dV curves are marked by arrows. (a–d) Reproduced with permis-
sion.[179] Copyright 2012, Nature Publishing Group. e) Band alignment of monolayer semiconducting TMDs and monolayer SnS2. Conduction band min-
imum (CBM) and Valence band maximum (VBM) calculated by Perdew-Burke-Ernzerhof (PBE) spin-orbital coupling (SOC) are indicated by the filled gray
columns, with G: the Green function of electron, W: the screened Coulomb potential (GW) corrected band edges indicated by the narrower olive columns.
Reproduced with permission.[156] Copyright 2013, American Institute of Physics. f,g) Charge densities of VBM (f) and CBM (g) states for the monolayer WX2–
MoX2 lateral heterostructures with common X. Reproduced with permission.[157] Copyright 2013, American Institute of Physics. h) Schematic, optical images
of monolayer and bilayer MoS2 with different twist angles. i) Calculated values for the Kohn–Sham K-valley direct bandgap (orange) and indirect bandgap
(dark yellow) for the energetically favorable structures at each twist angle. (h, i) Reproduced with permission.[181] Copyright 2014, Nature Publishing Group.
indicates that the electronic structures of graphene can be layer for θ = 0°, and Se atoms of top layer are on top of the
modulated by stacking it on hBN layers and the density of states metal atoms of the bottom layer for θ = 60°. They found that
in graphene layer for the new Dirac point can be determined the intensities of the PL excitonic peaks of the hetero-bilayer
by the mismatch between the graphene and hBN layers. The are one order of magnitude weaker than those of each mate-
electronic structures can also be modulated by the stacking of rial and the peaks show slightly redshift. The PL quenching in
different TMDs. Several groups have demonstrated that mon- the hetero-bilayer may result from the decrease of PL quantum
olayer MoX2–WX2 (X = S, Se, or Te)-based vdWHs have type-II yield in the case of bilayer systems and the redshift of the
band alignments by theoretical calculations and experiments vdWH may be attributed to the changes in the band structure.
(Figure 4e).[117,157,173,180] Because the optically active states of the More interestingly, a new peak at ≈1.35 eV was observed, which
conduction minimum and valence maximum bands are local- may be related to interlayer excitons based on band alignment
ized on opposite layers, the lowest energy electron–hole pairs are in Figure 5e. Generally, the d orbitals of W and Mo dominate
spatially divided, which is beneficial for the applications in solar the energy levels of WSe2 and MoSe2. The energy of 4d orbital
energy conversion and optoelectronics (Figure 4f).[157] Li and of Mo is lower than that of 5d orbital of W, thus the valence
co-workers[173] have experimentally verified that the MoS2–WSe2 band and conduction band of MoSe2 are lower than those of
heterostructure shows the conduction and valence band offsets WSe2, resulting in type-II band alignment between the hetero-
of 0.76 and 0.83 eV, respectively, which suggests a type-II band bilayer system. Under light illumination, electron–hole bound
alignment. On the contrary, Cho and co-workers[156] found that pairs (excitons) are generated in individual WSe2 and MoSe2.
vdWHs based on monolayer n-type MX2 (M = Mo, W; X = Se, Te) The energy levels of the excitons located between the conduc-
and p-type MX2 (M = Zr, Hf; X = S, Se) are calculated to be tion band and the valence band in each layer are due to their
promising couples realizing broken gap junctions with excel- less energy than the unbound electrons and holes. Then, the
lent electron tunneling efficiencies, which is of great interest for photoinduced electrons and holes are separated, and migrated
low-power logic devices. Monolayer 2D TMDs such as MoSe2, to the conduction band of MoSe2 and the valence band of
MoS2, WSe2, WS2 are direct bandgap semiconductors,[118] while WSe2, respectively. Consequently, the holes in the valence band
it transforms to indirect bandgap semiconductors as the layer of WSe2 and the electrons in the conduction band of MoSe2
number increases due to the Γ point to an intermediate state recombined to form interlayer excitons, resulting in interlayer
(Γ–Q) becoming non-negligible.[181] Furthermore, the electronic excitonic emission. Furthermore, they found that the PL inten-
properties of the vdW-stacked bilayer homostructure can be mod- sity of the interlayer excitonic emission reached the maximum
ulated by changing the interlayer distances or twisting the layers. at 0° and 60° and reduced at other twist angles (Figure 5f). The
Wang and co-workers[181] realized MoS2 bilayers with different hetero-bilayer system possesses highly symmetric stacking con-
twist angles as shown in Figure 4h, and they found that the indi- struction with strong interlayer coupling at 0° and 60°, thus
rect bandgap size varies evidently with the twist angles: it shows high charge transfer efficiency could be realized due to the
the largest redshift for AB (S atoms on top of the S atoms of the minimum interlayer distance, resulting in the higher PL inten-
bottom layer)- and AA (S atoms on top of the Mo atoms of the sity. This result provides a new degree of freedom to modulate
bottom layer)-stacked bilayers, while a significantly smaller and the optical properties of vdWHs with rich functionalities.
constant redshift for all other twist angles (Figure 4i). Many vdWHs based on TMDs form type-II band
Raman, PL, and absorption spectra, and exciton dynamics are alignments,[111,118,180] resulting in highly efficient electron–
the optimum methods to probe the optical properties of vdWHs hole separation, which is beneficial for light harvesting and
due to the efficient, accurate, and nondestructive measure- detecting.[197,198] Thus, exciton dynamics using pump–probe
ments.[182–196] Javey and co-workers[76] fabricated vdWH based on technique is booming development to probe the charge transfer
monolayer WSe2 and MoS2 and a distinguished PL peak at 1.55 process. Wang and co-workers[196] observed the ultrafast charge
eV (Figure 5a) was observed, which is lower than both the exci- transfer in the photoexcited monolayer MoS2/WS2 heterojunction
tonic PL peaks at 1.87 and 1.64 eV for the monolayer MoS2 and by employing both femtosecond pump–probe and PL mapping
WSe2, respectively. Furthermore, the absorption spectrum of the spectroscopy (Figure 5g). They found dramatical quenching effect
vdWH exhibits two absorption peaks at 1.91 and 1.65 eV in accord- of PL spectrum at the heterojunction compared with that at the
ance with the absorption peaks of individual monolayer MoS2 and individual single layer material (Figure 5h), suggesting the high
WSe2, respectively (Figure 5b). Interestingly, the vdWH shows efficiency of interlayer charge transfer. They further investigated
a prominent shift of ≈100 meV between the absorbance and PL the transient absorption spectra of the MoS2–WS2 heterojunction
peaks in Figure 5b, and this large Stokes-like shift confirms the from 2.0 to 2.5 eV (Figure 5i), and determined a hole transfer time
spatially indirect transition in a staggered gap (type-II) heterostruc- of ≈50 fs from MoS2 to WS2 layer. Such ultrafast charge transfer
ture. When illuminating light on the heterostructure, the photo- in vdWHs can promise the applications in photodetectors and
excited excitons relax at the interface, driven by the band offset in solar energy conversion. Zhao and co-workers[199] confirmed the
Figure 5c. The PL excitonic peak energy is lower than the excitonic coherent nature of interlayer charge transfer in a trilayer of MoS2–
bandgaps of each material due to the energy lost to the band offset. WS2–MoSe2 heterostructure. Excited electrons in MoSe2 transfer
They also found that the interlayer coupling can be effectively to MoS2 in 1 ps at room temperature without accumulation in the
modulated by inserting dielectric hBN layers into the vdW gap. middle WS2 layer, which indicates a coherent electron transfer pro-
Furthermore, Shin and co-workers[187] systematically investi- cess. Not only that, the WS2 layer separated the electron–hole pairs
gated the interlayer coupling between WSe2- and MoSe2-based and extended their lifetime to ≈1 ns. This trilayer vdWH configu-
vdWHs with different twist angles. As illustrated in Figure 5d, ration with long carrier lifetime and efficient charge transfer may
Se atoms of top layer are on top of the Se atoms of the bottom provide new applications in electronic and optoelectronic devices.
Figure 5. a) PL spectra of single-layer WSe2, MoS2, and the corresponding hetero-bilayer. b) Normalized PL (solid lines) and absorbance (dashed
lines) spectra of single-layer WSe2, MoS2, and the corresponding hetero-bilayer. c) Band diagram of WSe2/MoS2 hetero-bilayer under photoexcitation.
(a–c) Reproduced with permission.[76] Copyright 2014, National Academy of Sciences of the United States of America. d) Schematic front and side view
of the MoS2/WSe2 heterostructures with different twist angles. e) Excitonic band alignment of the MoSe2/WSe2 heterostructures under photoexcitation.
f) Intensity of the interlayer exciton peak versus the twist angle. (d–f) Reproduced with permission.[187] Copyright 2017, American Chemical Society.
g) Schematic illustration of the MoS2/WS2-based heterostructure. h) PL spectra of the isolated MoS2-, WS2-, and MoS2/WS2-based heterostructure.
i) 2D plots of transient absorption spectra at 77 K from a MoS2/WS2 heterostructure and an isolated MoS2 monolayer upon excitation of the MoS2
A-exciton transitions. (g–i) Reproduced with permission.[196] Copyright 2014, Nature Publishing Group.
4. Optoelectronic Applications of vdWHs monolayer MoS2-based transistor, which may result from the
same excited state (exciton A).[210] However, the EL emission
Since the tunable band alignments and strong light–matter limited at the metal contacts results in low quantum efficiency
interactions, the vdWHs provide a new platform for the appli- (10−5 for monolayer MoS2). Constructing p–n diode (LED) is an
cations in optoelectronics.[200–207] In this part, we will focus effective way to improve the EL efficiency. There are already lots
on those recently reported LEDs, photodetectors, and optical of reports on the LEDs based on 2D heterostructures, showing
modulators with novel constructions and mechanisms different high performances as summarized in Table 1. The lateral p–n
from those conventional devices. junctions in monolayer TMDs by the dual-gating tactic have
been successfully demonstrated recently with the active area
localized at the depletion region.[198,211–213] In contrast, vertical
4.1. Light-Emitting Diodes vdWHs have arised up for efficient carrier injection in LED
due to the large active area over the whole overlapping junc-
Monolayer TMDs are promising candidates for light emit- tion.[203,214,215] For example, Duan and co-workers[203] have
ting due to their direct bandgaps from visible to near-infrared investigated the EL properties based on p-WSe2/n-MoS2 diodes
range.[208,209] Electroluminescence (EL) can be observed in (Figure 6a). An EL image (Figure 6b) obtained under a forward
Table 1. Summary of typical heterostructure-based LEDs (Gr: graphene).
Device Vds Emission wavelength Line width Luminance Quantum efficiency References
[V] [nm] [meV] [cd cm−2] [%]
Gr/hBN/WSe2/hBN/Gr 2 759 0.2 [216]
hBN/WSe2/hBN 2.8 730 5 [218]
Gr/hBN/WSe2/hBN/Gr 720 20 [202]
Gr/hBN/WSe2/hBN/Gr 1.94 727 0.3 [204]
p-MgNiO/perovskite/n-MgZnO 5.5 522 3.8 × 103 2.39 [353]
Gr/WS2/hBN 640 80 [226]
p-WSe2/n-WSe2 733 5 [212]
n-MoS2/p-MoS2/p-GaN 4 White light 3.0 × 104 29 [201]
MoS2/Si 5.5 685 [215]
p-WSe2/i-WSe2/n-WSe2 750 10−2 [213]
p-WSe2/n-WSe2 800 0.1 [198]
p-WSe2/n-WSe2 2 750 0.1 [211]
Al2O3/MoS2/GaN 10−2 [31]
hBN/Gr/hBN/WSe2/hBN/MoS2/ −2.3 750 5 [74]
hBN/Gr/hBN
Gr/hBN/WS2 7 612 1 [217]
bias of 3 V exhibits that the EL signal is mainly from the over- of hot minority carriers to n-doped WS2 by Fowler–Nordheim
lapping area near the metal electrodes, which is significantly tunneling, with hBN blocking the hole- and electron-transport.
contrasting to the photocurrent mapping generated from the Therefore, Novoselov and co-workers[74] have created efficient
whole overlapping area. For photocurrent mapping under small LEDs employing graphene as transparent conductive layers,
bias lower than turn-on voltage, the resistance of the p–n junc- hBN as tunneling barriers, and different TMDs as quantum
tion governs the entire diode, and thus the photocurrent can walls (QWs) as shown in Figure 6c. In these devices, electrons
be observed from the whole overlapping area. However, EL is and holes are injected into the TMD layer from the two gra-
measured at a higher bias exceeding the turn-on voltage of the phene electrodes. These kinds of vertical heterostructures allow
diode, and the entire resistance is gradually dominated by that of brighter LEDs (Figure 6c) due to the reduced contact resistance
monolayer WSe2. Thus, the most voltage drop generates across and higher current densities. For example, the PL of MoS2-
the heterojunction edge near the electrodes. It is observed that based single QW is dominated by the neutral A exciton at
the EL intensity increasing as a function of injection current 1.93 eV at low bias. There are also two weaker and broader peaks
exhibits a distinct threshold. Under small forward bias lower at 1.79 and 1.87 eV attributed to bound excitons. However, the PL
than the certain threshold, the holes from WSe2 are injected spectrum changes dramatically and exhibits a new peak at 1.90 eV
into MoS2, while few electrons can flow from MoS2 to WSe2 due at a certain gate voltage. This transition may be caused by the
to the barrier. Thus, the radiative recombination in MoS2 is very Fermi level of the bottom graphene rising above the conduc-
weak due to the indirect bandgap of the few-layer MoS2. With tion band of MoS2, resulting in electrons flowing into the QW.
further increasing of the bias higher than the threshold, both The obtained quantum efficiency can reach ≈10% which is
the electrons and the holes can go through the junction and are ten times higher than that of planar p–n diodes[198,211,212] and
injected into p-type and n-type regions due to the upward shift 100 times higher than that of Schottky barrier diodes.[210] They
of the conduction band of MoS2. Then, the EL is dominated by further introduced multiple QWs stacked in series to increase
the radiative recombination in WSe2 and increases linearly with the probability for injected carriers to radiatively recombine.
the injection current. Notably, fitting the EL spectra via multiple Besides, monolayer TMDs are mostly direct bandgap semicon-
Guassian functions, two hot electron luminescence peaks at ductors and possess a large range of bandgaps, which are prom-
≈546 and ≈483 nm are also observed, which could be employed ising for atomically thin white LEDs. Chen and co-workers[201]
to probe the electron–orbital interaction in WSe2. In order to fabricated the white LED employing n-MoS2/p-MoS2/p-GaN as
reduce the leakage current in the vertical stacking structures, the orange, green, and blue emitters, respectively. White LED
functional stacking structures for light emission are developed has promising applications in lighting and display due to high
by inserting tunneling layers (such as hBN, Al2O3) into the p–n brightness for low-power consumption and long lifetimes for
junction and/or the electrode contacts, which enables the long high-performance operation. Thus, a heterostructure based on
lifetime of excitons in TMD quantum wells.[31,74,202,216–219] For n-MoS2/p-MoS2/p-GaN has been fabricated with the EL spectra
example, planar EL from tunnel diodes based on a metal–insu- at 642 nm (n-MoS2, orange), 525 nm (p-MoS2, green), 481 nm
lator–semiconductor vdWH consists of few-layer graphene, (p-GaN, blue), showing the potential to fabricate atomically thin
hBN, and monolayer WS2, showing an excellent quantum effi- light sources with white LED.[201] Besides, thermal light emis-
ciency of ≈1%.[217] The light emission is realized by the injection sion from graphene[220] and MoS2[221] has also been realized
Figure 6. a) Schematic diagram of the WSe2/MoS2 heterostructure. b) The false-color EL image of the heterojunction device under an injection current
of 100 µA. (a, b) Reproduced with permission.[203] Copyright 2014, American Chemical Society. c) Schematic of the single quantum wall heterostructure
hBN/graphene/2hBN/WS2/2hBN/graphene/hBN, and the optical image of EL from the same device. (c) Reproduced with permission.[74] Copyright
2015, Nature Publishing Group. d) Schematic of the arrangement of the heterostructure. e) PL and EL spectra of the heterostructure. Inset: Schematic
illustration of the carriers’ transportation. (d, e) Reproduced with permission.[222] Copyright 2017, American Chemical Society. f) Schematic of the
vertical heterostructure LED operation. (f) Reproduced with permission.[204] Copyright 2017, American Chemical Society. g) Schematic drawing of the
device. (g) Reproduced with permission.[205] Copyright 2016, American Chemical Society.
with enhanced bright light emission via suspended device, the small electron–hole wave function overlap in XI, XI domi-
which may pave the way toward the realization of commercially nates the radiative recombination. In brief, most of the holes
viable large-scale, atomically thin, flexible, and transparent light in the valence band of WSe2 and the electrons injected into
emitters and displays with low operation voltage. the conduction band of MoSe2 meet at the junction, and bind
Most vdWHs exhibit type-II band alignment, resulting in to XI due to the strong Coulomb interaction, and then recom-
efficient separation of electron and hole pairs. However, the bine to emit light. Quantum emitters resulting from quantum
spatially isolated electrons and holes still undergo strong Cou- confined structures (such as quantum defects and dots) may
lomb interaction due to the small interlayer isolation, resulting induce single photons, which is crucial for applications in
in tightly bound interlayer exciton (XI).[69] Thus, Xu and quantum information and high-resolution metrology. TMD
co-workers[222] electrostatically constructed lateral p–n diode quantum emitters with a very sharp photon emission spectrum
based on the MoSe2–WSe2 hetero-bilayer to probe the EL prop- have been successfully fabricated.[224–228] For example, Xu and
erties (Figure 6d). The PL spectrum in Figure 6e illustrates that co-workers[204] constructed the heterostructure composed of
many peaks from 1.56 to 1.74 eV in both MoSe2 and WSe2 relate two stacked graphene layers as electrodes, separated by thin
with the intralayer A exciton, neutral, charged, and localized WSe2 layer with hBN as barriers, as shown in Figure 6f. The
excitons. The dominant emission below 1.4 eV is fingerprint Fermi level of the graphene layers lies between the bandgap of
of the interlayer exciton. However, the EL spectrum is deter- WSe2 under no external bias. While, the Fermi level rises above
mined by the interlayer emission, with only a small intralayer the available subgap defect states as the device biased. Conse-
signal at 1.62 eV, probably the MoSe2 trion.[223] Thus, though quently, electrons (holes) can tunnel through the hBN barriers
the energy of XI is lower than that of intralayer exciton due to to WSe2 with increased bias and the carriers are expected to
form bound excitons due to the strong Coulomb interactions. Photodiodes based on n-type MoS2, p-type BP and WSe2
Then, the excitons recombine, resulting in EL from intrinsic have been recently constructed.[70,203,234] However, most of them
along with defect-bound excitons. Furthermore, a broad peak show poor external quantum efficiencies (EQEs) such as 0.3%
(1.651–1.71 eV, marked as Xd) at lower energy than the intrinsic for BP/MoS2 and 12% for WSe2/MoS2, respectively. Then, He
excitons becomes dominant. They further demonstrated that and co-workers[235] constructed photodiodes based on p-GaTe/n-
the emission originates from spatially localized regions of the MoS2 (Figure 7a), and acquired a high EQE of 61.68%. To fur-
sample, and the EL spectra from single defects have a doublet ther investigate the transport mechanism, they have measured
with the characteristic exchange splitting and linearly polar- the low temperature electrical properties. Thus, they found the
ized selection rules. Kis and co-workers[205] introduced spin interlayer recombination dominated by the Shockley–Read–
injection from a ferromagnetic electrode into a heterostructure Hall (SRH) recombination, and a negative temperature gradient
based on monolayer WSe2/MoS2 and the spin-polarized holes of (dVoc/dT) ≈ −0.7 mV K−1. Kim and co-workers[214] fabricated
in WSe2 transporting laterally, resulting in circularly polarized vertical heterostructures based on atomically thin MoS2 and
light emission that can be modulated by external magnetic field WSe2 in Figure 7b. They found that most of the voltage drop
(Figure 6g). Because the energy of the valence band at Γ point at the vertical junction, with negligible potential barriers along
is 0.5 eV lower than that at the K–K′ point in monolayer WSe2, the lateral transport direction under forward bias, contrary with
resulting in the spin injection occurring at the K–K′ point. potential barriers resulting from band bending in the lateral
Then, those spin-polarized holes recombine with unpolarized direction under reverse bias. Thus, the tunneling-assisted inter-
electrons from MoS2 at the heterojunction area. Due to the layer recombination may determine the current under forward
breaking inversion symmetry, the electronic states in the K and bias. This unusual interlayer recombination may be related
K′ valleys exhibit different chiralities and the interband transi- to two physical mechanisms or a merging of them: (a) SRH
tions at band edges involve σ+ and σ− polarized light. The tran- recombination assisted by inelastic tunneling of majority car-
sition energy can also be tuned by the external magnetic field riers into trap states in the gap; (b) Langevin recombination by
through the valley Zeeman effect. These ingenious strategies Coulomb interaction. Furthermore, the large band offset for
such as the bound interlayer excitons, single defect emitters, conduction bands (∆EC) and valence bands (∆EV) at the junc-
spin injection employed to realize atomically thin LEDs provide tion could promote the efficient separation of the photoexcited
new opportunities for the next-generation LEDs. electron and hole pairs. Generally, the charge transfer processes
in the ultrathin p–n junctions are efficient and fast due to the
forbidding of the exciton (or minority carriers), which are con-
4.2. Photodetectors firmed by the observation of the PL quenching and the genera-
tion of photocurrent in the p–n junction. Besides, the inter-
Photodetector is a fundamental building block of many layer tunneling-assisted recombination also acts as a key role
devices in our daily life such as environment monitoring, in determining the photoresponse. Because the photocurrent
video imaging, military, remote sensing, optical communica- is dominated by the difference between the gate-independent
tions, and so on.[115,229] 2DLMs exhibit excellent properties generation rate and the recombination rate, the prominent
such as high transparency, strong light–matter interaction, peak of the photoresponse can be experimentally fitted by both
flexibility, and facile integration with current complementary the SRH and Langevin recombinations (Figure 7c). Though
metal–oxide–semiconductor technology. Furthermore, vdWHs Langevin recombination may play a key role here due to the
based on diverse 2DLMs provide more tunability for the band enhanced Coulomb interaction between the electrons and the
alignments, carrier densities, resulting in multifunctional het- holes confined in the 2D systems,[236] SRH recombination
erostructures and show promising applications in high per- could still affect the process due to the defects at the interface.
formance photodetectors. Thus, diverse photodetectors based Duan and co-workers[237] illustrated a graphene/MoS2/gra-
on 2D heterostructures exhibiting high performances or novel phene vertical heterostructure (Figure 7d). The heterostructure
constructions have been reported (Table 2). This section briefly shows clear photoresponse with a short-circuit current of ≈2 µA
introduces the photodetection mechanisms of the electron–hole and an open-circuit voltage of ≈0.3 V (Figure 7e) and the photo-
separation and the extended applications. current mapping of the vertical heterostructure suggests photo
current generated over the entire heterostructure. The whole
photocurrent increases and the area of photoresponse also
4.2.1. Photovoltaic Effect extends to the overlapping area of the top and bottom graphene
with the gate decreasing, which indicates that the photoexcited
In the photovoltaic effect, photoexcited electron–hole pairs carriers outside the vertical junction can also contribute to the
are separated by the built-in electric field which is generated total photocurrent and the diffusion length of the minority car-
at the p–n junction. In this case, the Ids–Vds curves show non- riers in this device is at least on the micrometer scale. They also
linear characteristics in dark. Under illumination and without found that generation, separation, and transport processes of
external bias (Vds = 0), the built-in electric field separates the the photoexcited carriers in the stacked device can be modulated
photogenerated electron–hole pairs, thus resulting in a meas- by the back-gate voltage. The Schottky barrier height difference
urable photocurrent (short-circuit current, Isc). The carriers of between top graphene–MoS2 and bottom graphene–MoS2 con-
opposite polarities in distinct parts of the device accumulate tacts dominates the original built-in potential. A monotonic
with the circuit opening, and thus a voltage is generated (open band slope across the whole vertical junction is formed through
circuit voltage, Voc).[197,230–233] the merging of the top and bottom Schottky barriers, due to the
Table 2. Summary of typical 2D vdWH-based photodetectors (GO: graphene oxide).
Device Iph/Idark Responsivity EQE Rise time Specific detectivity References

[A W−1] [%] [ms] [Jones]
BP/MoS2 0.4 0.3 [70]
WSe2/BP/MoS2 6.3 1.25 × 1011 [265]
MoS2/BP 103 22.3 1.5 × 10−2 3.1 × 1011 [354]
InSe/Gr 4× 103 3.1 × 10 3 [355]
MoTe2/MoS2 0.3 85 [356]
PbS/Gr 2.5 × 106 24 [102]
SnS2/MoS2 50 1.3 264 [90]
MoS2/hBN/Gr 105 180 230 2.6 × 1013 [245]
WS2/MoS2 103 1090 6.9 3.5 × 1011 [357]
MoTe2/MoS2 2 0.06 1.6 × 1010 [149]
CdS/MoS2 3.9 100 [101]
−2
GaSe/GaSb 0.1 50 3.2 × 10 2.2 × 1012 [358]
MoS2/GaAs 0.3 1.7 × 10−2 3.5 × 1013 [359]
WSe2/MoS2 12 [203]
−2
WSe2/MoS2 1.1 × 10 1.5 [234]
Gr/hBN/MoTe2 610 3.3 × 1011 [166]
MoS2/hBN/Gr 6.6 3 × 10−4 10 [167]
MoS2/Gr/WSe2 4250 106 5.3 × 10−2 2.2 × 1012 [267]
GaTe/MoS2 21.8 61.6 8.4 × 1013 [235]
PbS/MoS2 130 4.5 × 104 7.8 3 × 1013 [103]
SnSe2/BP 2.4 × 10−4 [244]
Gr/MoS2 2 × 103 1.5 × 1010 [360]
ReSe2/MoS2 6.7 1.2 × 103 [361]
WSe2/GaSe 6.2 1.4 × 103 3 × 10−2 [207]
GaSe/InSe 103 9.3 2 × 10−3 [362]
WSe2/MoS2 0.1 2.4 [214]
hBN/WSe2/hBN 7.3 1.5 × 10−9 [363]
Gr/MoS2 5 × 108 80 [364]
Gr/MoS2/Gr 0.2 55 [237]
Gr/WS2/Gr 30 [64]
GO/Si 104 1.5 2 [365]
BiI3/WSe2 1.6 1.4 [231]
MoTe2/Gr 970.8 [366]
Gr/MoS2 45.5 [257]
SnSe2/MoS2 9.1 × 103 3.1 × 104 200 9.3 × 1010 [95]
shorter channel length (≈50 nm) than the total depletion length and co-workers[238] employed an organic small molecular p-type
(≈140–170 nm). Thus, this band slope dominates the generation pentacene and n-type MoS2 for constructing type-II photovol-
and separation of the excited carriers. Herein, because of the taic devices (Figure 7f). Furthermore, they employed transient
p-type doping of graphene by the substrate, the Schottky bar- absorption spectroscopy to probe the kinetics of the excited
rier height in top graphene–MoS2 is lower than that in bottom carriers.[239] The results illustrate that the separation of MoS2 exci-
graphene–MoS2, which leads to the fact that a built-in potential tons occurs by hole transferring to pentacene in 6.7 ps, and the
propels photoexcited electrons to the top graphene. The EQE of charge dissociation extends to 5.1 ns, which is at least one order
the device can reach up to ≈27%, which is much higher than of magnitude longer than the recombination lifetimes from
many heterostructures based on TMDs.[70,203] A much larger those 2D heterostructures reported previously.[69,196] They dem-
and tunable band offset leading to efficient charge separation onstrated a concept of an organic–2D MoS2 heterostructure and
may partially explain the high EQE. On the other hand, Lauhon the semiconducting polymer that could offer high performance
Figure 7. a) Schematic of GaTe/MoS2 vdWH. (a) Reproduced with permission.[235] Copyright 2015, American Chemical Society. b) Bottom left: Sche-
matic diagram of a vdW-stacked MoS2/WSe2 heterojunction device with lateral metal contacts. Top: enlarged crystal structure, with purple, red, yellow,
and green spheres representing Mo, S, W, and Se atoms, respectively. Bottom right: Optical image of the fabricated device. Scale bar: 3 µm. c) Measured
(circles and dashed curve) and simulated (green curve for 2D Langevin process and purple curve for SRH mechanism) photocurrent at Vds = 0 V as
a function of gate voltages. For the fit, B = 4.0 × 10−13 m2 s−1 and τ = 1 µs are used for the 2D Langevin (s = 1.2) and SRH mechanisms, respectively.
(b, c) Reproduced with permission.[214] Copyright 2014, Nature Publishing Group. d) Schematic illustration of the device layout. e) I–V curves under dark
and illumination. (d, e) Reproduced with permission.[237] Copyright 2013, Nature Publishing Group. f) Schematic diagram of the device. (f) Reproduced
with permission.[238] Copyright 2016, American Chemical Society.
in large-scale devices, which is possibly compatible with the energy. Exploiting the redundant thermal energy in the elec-
technology of nanoelectronics and optoelectronics. tron bath is a prospective way to conquer these restrictions.
This energy comes from the thermalization of photoexcited
carriers, resulting in a the hot carrier distribution with a well-
4.2.2. Photo-Thermoelectric Effect determined temperature Te. More carriers can break through
the Schottky barrier with increasing Te, generating a current
Photo-thermoelectric effect appears with the nonuniform via thermionic emission. On this occasion, even photons with
heating by light-induced temperature gradients, resulting in a the energy lower than the Schottky barrier could make the Te
photocurrent or photovoltage. Thus, the two ends of the semi- increase and thus carrier emission. Koppens and co-workers[241]
conductor show a temperature difference, resulting in a voltage fabricated vertical heterostructure based on graphene/WSe2/
difference (photo-thermoelectric voltage, VPTE) via the Seebeck graphene to detect low-energy photons (a wavelength up to
effect. And, the VPTE can be presented by: VPTE = (S1 − S2)ΔT, 1500 nm) via photo-thermionic emission (Figure 8a). Graphene
where S1, S2 are the Seebeck coefficients of the two matters, ΔT absorbed the photons creating electron–hole pairs. Then, the
is the temperature difference. Notably, the photo-thermoelectric electron–hole pairs quickly equilibrate into a thermalized car-
effect is sparse in a popular semiconductor due to negligible rier distribution with an increasing Te. Carrier in this spreading
temperature gradients.[229,240] Successful execution of this tac- with higher energy than the Schottky barrier height at the
tics needs a broadband absorber where the interaction of car- graphene/WSe2 interface could transfer through the WSe2
riers themselves is stronger than with phonons, along with layer and further move to the graphene layer on the other side
energy-selective contacts to acquire the excess electronic heat. (Figure 8b). The photocurrent generated in the sub-bandgap
Generally, the photoexcited carriers (or hot carriers) transfer a range illustrates a prominent superlinear dependence on laser
Schottky barrier between a semiconductor and an electrode, power (Figure 8c), which confirms the thermal emission of car-
allowing detection of photons with lower energy than the riers through the Schottky barrier. They further employed gate
bandgap of the semiconductor, which promote the applica- voltage to enhance the photocurrent via modulating the height
tions in the visible and near-infrared photodetectors. However, of graphene/WSe2 Schottky barrier through controlling the
if the photon energy is lower than the Schottky barrier, the Fermi level of graphene. Time-resolved photocurrent measure-
efficiency of this mechanism will drop and will be restricted ments are employed to further confirm the sub-bandgap photo-
by the ability to extract the carriers before losing their initial current coming from the photo-thermionic effect (Figure 8d).
Figure 8. a) Schematic representation of the heterostructure, to which a gate voltage (Vgs) is applied to modify the Fermi level of the bottom graphene.
An interlayer bias voltage between the top and bottom graphene flakes can be applied. b) Simplified band diagram of the photo-thermionic effect at a
graphene/WSe2 interface. c) Power dependence of the photocurrent for various values of photon energy. d) Time-resolved photocurrent change. Inset:
The same data and fit in logarithmic scale. (a–d) Reproduced with permission.[241] Copyright 2016, Nature Publishing Group.
The extracted characteristic decay time of 1.3 ps is on the order valence band in BP have a maximal overlap with the occupied
of the cooling time of hot carriers in graphene.[242,243] These states of conduction band in SnSe2. Further increase of the for-
results verify the photo-thermionic effect dominating the gener- ward bias results in the alignment of the forbidden bandgap
ation of photocurrent. Applying a positive gate voltage effectively of BP with the occupied conduction band states. Though the
reduces the Schottky barrier height due to the bottom graphene tunneling probability increases slightly due to a stronger elec-
doped by electrons, resulting in a strikingly enhanced photo- tric field, the tunneling current decreases. The device current
current. Thus, the photoresponsivity can reach 0.12 mA W−1 acquired its minimum value dominated by a combination of
at wavelength of 1500 nm, and the translated internal quantum phonon-assisted tunneling and thermionic current, and then
efficiency is 2%. increases due to the overriding thermionic current. They
further probed the photoresponse of the tunneling diode
(Figure 9c). The photocurrent and photovoltage are closely
4.2.3. Tunneling Effect related to the energy band bending in the heavily doped p+
and n+ regions near the junction due to the perfect Ohmic
Interband tunneling in adjacent semiconductors has attracted contact near zero bias. The photocurrent will drive the I–V
intensive attention as a new kind of transistors owing to the curve to the second quadrant with the carriers accumulation
promising applications in low-power consumption devices. near the junction as shown in the inset of Figure 9c. Whereas,
Xing and co-workers[244] integrated p-BP and n-SnSe2 for the photocurrent will drive the I–V curve to the fourth quad-
constructing the Esaki diode (Figure 9a). The accumulation rant as a typical p–n diode with the carrier depletion near the
of electrons in SnSe2 and holes in BP occur around the junc- junction. Thus, the responsivity of the device can be estimated
tion due to the large work function difference (Figure 9b). to be ≈0.24 mA W−1.
Electrons flow from the conduction band of n-SnSe2 into the Yu and co-workers[245] reported a highly sensitive hetero-
empty valence band states of p-BP via tunneling through the structure based on MoS2/hBN/graphene by introducing hBN
barrier under a small forward bias. This tunneling current as the tunneling barrier (Figure 9d). The I–V curves in this
achieves its maximum value when the unoccupied states of device can be fitted by the direct tunneling (DT) at low voltage
Figure 9. a) Optical image of the BP/SnSe2 heterostructure. b) Id–Vds curves at 80 and 300 K in a linear scale. c) Id–Vds curves under dark and illumi-
nation with different laser powers. (a–c) Reproduced with permission.[244] Copyright 2015, American Chemical Society. d) Schematic diagram of the
electron–hole pair generation and tunneling across the barrier. e) I–V characteristics of the device under dark and various illumination intensities of
the 405 nm laser. f) Energy band diagrams of the MoS2/hBN/graphene heterostructure at flat band model. (d–f) Reproduced with permission.[245]
Copyright 2017, American Chemical Society. g,h) Schematic images of the graphene/1-layered MoS2/graphene and graphene/7-layered MoS2/graphene
heterostructures with SiO2 substrate and air environment, respectively. i) Electrostatic potentials of the graphene/1L-MoS2/graphene heterostructures
including environmental condition. (g–i) Reproduced with permission.[246] Copyright 2016, Nature Publishing Group.
while Fowler–Nordheim tunneling (FNT) at high voltage from the I–V curves under dark and illumination, resulting in
(Figure 9e). DT and FNT can be presented by the following the band alignments in Figure 9f. At forward bias under dark,
equations the DT of electrons is severely impeded by the high trapezoidal
h-BN barrier, leading to ultralow dark current. Although the tri-
A mϕ B q 2Vds  −4 π m *ϕ d  angular hole barrier at the MoS2/hBN junction is lower than
I DT (V ) = 2
exp  B
 (1) the trapezoidal graphene/hBN barrier, a negligible FNT current
hd  h 
occurs due to lacking of minority hole carriers in MoS2. How-
ever, when light is illuminated on the device, large amounts
 −8 π 2m *ϕ B3/2d  of electron–hole pairs are generated in MoS2, resulting in a
Aq 3mVds2
I FNT (V ) = exp   (2) dramatic increase in hole tunneling across the triangular hole
8 π hϕ Bd m
2 *
 3hqVds  barrier at MoS2/hBN. Thus, the tunneling mechanism domi-
nated phototransistor can show a high detectivity of 2.6 × 1013
where A, d, h, m, ϕB, m*, and q are the effective contact area, Jones as well as a high responsivity of 180 A W−1. Duan and
the thickness of hBN, the Planck’s constant, the free electron co-workers[246] studied the layer-dependent photoresponse
mass, the barrier height, the effective electron mass, and the in graphene/MoS2/graphene-based vertical heterostructures
electron charge, respectively. Therefore, the barrier height at (Figure 9g,h). Interestingly, they found that the photorespon-
the graphene–hBN and MoS2–hBN interfaces, can be calculated sivity of monolayer MoS2 is several times higher than that in
seven-layer MoS2. In this device, the doping difference of the transferred electrons from MoS2 would occupy energy states
top and bottom graphene induces built-in voltage, resulting above EF (Figure 10g), thus decreasing the hole current in
in asymmetric barrier height between the top and bottom graphene. Higher p-type doping of graphene will promote
junctions (Figure 9i). Thus, the photoinduced electrons can electrons injection from MoS2 into graphene with a negative
effectively tunnel to lower barrier at the interface between gate bias (Figure 10g). Thus, the photoresponse is expected
the top graphene and MoS2, whereas the electrons tunneling to be enhanced, due to more photoexcited electrons into gra-
are blocked by the higher barrier at the interface between phene and contributing to photocurrent. While, the p-type
the bottom graphene and MoS2. Such asymmetric tunneling doping effect will reduce at a positive gate bias (Figure 10h).
induces photocurrent in the vertical heterostructure. The intro- The photoexcited electrons in MoS2 will become less attracted
duced quantum mechanical-based tunneling mechanism pro- by graphene due to the weaker built-in voltage field at the
vides a new view to probe the interaction in vdWHs and to fab- interface between MoS2 and graphene. Thus, the photore-
ricate the next-generation optoelectronics. sponse is expected to reduce. The flexible photodetector shows
a high photoconductive gain of ≈4 × 105, extending the appli-
cations to wearable devices.
4.2.4. Electrolyte Gate
Electrolyte gate can modulate the carrier density of the device 4.2.5. Broadband Photodetection
to a higher upper limit compared with that tuned by solid
state dielectric (up to 1013 cm−2). When the gate is applied on Current photodetection primarily depends on individual photo
the electrolyte solution, the ions in the electrolyte will move to active semiconductors with distinct bandgaps corresponding
the surface of the semiconductors and thus generate the elec- to their certain spectral scopes. Broadband photodetection is
tric double layer (EDL). Generally, the thickness of the EDL vital in many important optoelectronic applications such as
is extraordinarily thin (<1 nm). Thus, the carrier density can communication and imaging.[261–263] Most broadband photo-
reach up to 1014 cm−2 at small bias due to the large capacitance detectors reported are based on graphene or BP with narrow
of the electrolyte gate. The modulation of carrier density is sig- bandgaps, while poor photoresponsivities are usually observed
nificantly promising in tuning the performance of electronics due to the ultralow efficiency of the photoexcited electron
and optoelectronics.[142,158,247–255] Russo and co-workers[256] and hole pairs.[79,135,264–266] Recently, Miao and co-workers[267]
fabricated photodetectors based on WS2–graphene hetero- demonstrated an atomically thin heterostructure based on
structures encapsulated in an ionic polymer, lithium per- WSe2–graphene–MoS2 with sandwich structure (Figure 11a).
chlorate/poly(ethylene oxide), 8:1 in methanol) (Figure 10a). Graphene in the middle of the p–n heterostructure plays the
The generation of short-circuit photocurrent is localized to the vital role in wide spectral response range (Figure 11b). When the
lateral interface between Au and WS2, and varies in polarity illuminated photon energy is larger than the bandgap of mono
across the region of photoresponse (Figure 10b). Photocur- layer MoS2 (1.88 eV) and WSe2 (1.65 eV), all the three layers
rent exhibits a reduction under illumination and this sustains are photoactive materials which can generate large amount of
with more negative gate biases (Figure 10c). The mechanism photoexcited carriers, leading to high photoresponse. Whereas,
of photocurrent generation is the photogating effect: photoex- the interband absorption of MoS2 and WSe2 is forbidden when
cited electron–hole pairs are separated at the interface between the illumination photon energy is smaller than 1.65 eV. Then,
graphene and WS2, with one charge carrier moving to gra- graphene becomes the only absorption material to produce
phene while the other left in WS2 (Figure 10d). The difference electron–hole pairs, resulting in smaller photoresponse in the
of the work functions of graphene and WS2 promotes this sep- infrared range. In the visible range, the calculated detectivity
aration at the interface. Because of the recombination between can reach 1015 Jones and remains 1011 Jones in the near-infrared
electrons transferred from WS2 to graphene and the electro- range, which may provide a new platform for the atomically
statically induced holes in graphene, the resistance of the thin heterostructures applied in sensitive optoelectronics.
heterostructure increases at Vgs < VDirac under illumination. Duan and co-workers[268] further illustrated a type-II MoTe2/
This confirms the n-type doping in graphene. Thus, the photo- MoS2 vdWH exhibiting interlayer optical transition for the
gating effect-dominated photodetector shows a responsivity of infrared photodetection (≈1550 nm), which exceeds the spectral
≈1 × 106 A W−1, and a fast response of sub-milliseconds, sug- response limits of the intrinsic bandgaps of the composed sem-
gesting promising applications in video-frame-rate imaging iconductors (Figure 11c). Although the spectral response cutoff
applications. Ferrari and co-workers[257] illustrated a polymer wavelength of 1200 nm for monolayer MoTe2 and 700 nm for
electrolyte-gated MoS2/graphene grown by CVD method- monolayer MoS2, the interlayer gap from the valence band
based photodetectors, and employed a polyethylene terephtha- in MoTe2 to the conduction band in MoS2 is ≈0. 66 eV
late film as a flexible substrate (Figure 10e). At zero gate bias, corresponding to 1880 nm (Figure 11d). They theoretically
the band alignment is in the thermodynamic equilibrium as demonstrated that the electrons are localized in monolayer
demonstrated in Figure 10f, due to the electron affinity of MoS2, while holes are localized in monolayer MoTe2, sug-
monolayer MoS2 (≈4–4.2 eV)[258] lower than the Dirac point gesting the efficient charge separation in the heterostructure.
of graphene (≈4.6 eV).[259] The graphene is assumed to be The observation of interlayer optical transition in type-II vdWH
p-type doped.[260] Under illumination and voltage bias, photo could promote the understanding of the fundamental physics
excited electrons in MoS2 would transfer into graphene, and inspire novel construction of the next-generation infrared
with the uncompensated holes remaining in MoS2. The optoelectronics.
Figure 10. a) Device schematic with electrolyte gate. b) Scanning photocurrent map of a large-area device in short-circuit configuration. c) Ids–Vgs curves
under dark and illumination. d) Schematic image of charge transfer at the WS2/graphene interface. (a–d) Reproduced with permission.[256] Copyright
2017, John Wiley & Sons, Inc. e) Schematic of the graphene/MoS2 heterostructure with electrolyte gate. f–h) Schematic band diagram of polyethylene
(PE)-gated graphene/monolayer MoS2 Photodetector (PD) at (f) zero, (g) negative, and (h) positive Vgs. (e–h) Reproduced with permission.[257]
4.3. Optical Modulators system, including polarization controllers,[272] optical limiters,[273]

wavelength convertors,[274] and saturable absorbers.[275] Graphene
The optical modulator is employed for modulating the proper- enables the existence of resonant electron–hole pair with broad-
ties such as phase and intensity of the incident light,[269] and is band spectral range from visible to far-infrared. Because of the
one of the most crucial operations in photonics, showing prom- interaction between ultrafast optical pulses and charge carriers,
ising applications in optical interconnect, security, and medicine. a nonequilibrium carrier population in valence and conduction
2DLMs provide prospective opportunities for various multifunc- bands relaxes on an ultrafast timescale,[276] which enables wide-
tional photonics, which may be totally different from those based band and ultrafast saturable absorption from Pauli blocking. How-
on conventional bulk materials.[270,271] Optical modulation effects ever, graphene’s application at the end of the spectrum has been
in 2DLMs have been intensively explored recently. Consequently, impeded by the tremendous saturation fluence at wavelengths
massive prototypes of optical modulators with different modula- shorter than the near-infrared spectral region.[277] Different
tion mechanisms (such as all-optical, electro-optic, thermo-optic from graphene, TMDs[278] and BP[279] demonstrate bandgaps
modulations, and other modulation approaches) have been dem- for resonant light absorption in the visible and mid-infrared,
onstrated showing exciting performance. respectively.[280–283] Abundant attempts on 2DLM saturable
absorbers have exhibited exciting improvement of performance,
especially for ultrafast pulse generation.[277] For example, most
4.3.1. All-Optical Modulators reports have successfully demonstrated ultrafast pulse genera-
tion, improving pulse repetition rates up to 10 GHz,[284] pulse
All-optical modulation based on 2DLMs has been intensively widths down to sub-100 fs.[285] External cavity optical pro-
investigated with the signal processing realized in photonic cessing is also an effective way to improve the performance
Figure 11. a) Schematic of the WSe2/graphene/MoS2 heterostructure. b) Photoresponse and detectivity of the heterostructure at a wavelength range
from 400 to 2400 nm. (a, b) Reproduced with permission.[267] Copyright 2016, American Chemical Society. c) Schematic of the MoTe2/MoS2 heterostruc-
ture under illumination. d) Band diagram of the heterostructure with interband excitation process. (c, d) Reproduced with permission.[268] Copyright
2016, American Chemical Society.
such as the pulse duration, the wavelength accessibility, and Graphene shows weak second-harmonic generation due to
the output power and pulse energy.[277,285] Combining passive centrosymmetry.[296] However, other 2DLMs (such as WSe2,[297]
and active modulation function in 2DLMs is also a promising WS2,[298] hBN,[299] MoS2[300]) have exhibited strong second-order
way to further improve the ultrafast laser performance.[286] An nonlinearity with an odd number of layers due to the broken
all-optical modulator with a single-mode microfiber coated symmetry. High optical nonlinearity in 2DLMs shows highly
with graphene has been realized, exhibiting ≈2.2 ps response promising applications in quantum optical switches[301] and
time and 38% modulation depth.[287] In free-space set-ups, high-purity quantum emitters for integrated quantum circuits.
graphene–silicon heterostructure-based modulator shows a
wideband (0.2–2.0 THz) terahertz light modulation with a
maximum modulation depth of 99% via exploring the optical 4.3.2. Electro-Optic Modulators
doping effect.[288] Because of the fast response of the third-
order nonlinear susceptibility in graphene,[274,289] wavelength The electro-optic effect modulators are highly promising for
modulators based on atomically thin nonlinear optics is highly data communication link applications. Graphene is a prom-
promising for ultrafast all-optical information processing such ising material for optical modulator due to its tunable dielec-
as all-optical wavelength conversion. Whereas, several reports tric constant. Thus, many reported 2DLM-based electro-optic
on 2DLMs demonstrated that it is indispensible to improve the modulators are based on graphene.[13,270,302–307] Typical modula-
light–matter interaction due to the sub-nanometer thickness of tion speeds of electroabsorption modulators based on graphene
2DLMs and optical damage due to the high excitation power. at the visible and near-infrared range are on the order of giga-
Recently, many strategies have been proved to be helpful for hertz (≈1 GHz[13,308] and 30 GHz[309]). Though 2DLMs show
improving light–matter nonlinear optical interaction in 2DLMs strong light–matter interaction, the absolute value is very small
such as slow-light wave guides, microcavities, coherent con- for atomic-scale materials.[270,310] For example, monolayer gra-
trol, interference effects, doping, evanescent mode integration, phene can only absorb ≈2.3% of white light,[310] suggesting that
stacking multiple monolayers.[277,290–294] 2DLM-based hetero- the intrinsic modulation of monolayer graphene can only be up
structures such as MoS2–WSe2[295] and MoS2–WS2[196] have also to ≈0.1 dB. However, this value is far lower than ≈50% required
been demonstrated for new-type linear and nonlinear optical signal modulations for practical applications. Therefore, diverse
device constructions with tunable optical properties (carrier methods have been proposed to improve the modulation depth
dynamics and reflectance). However, 2DLM heterostructure- such as employing multilayer devices (few-layer graphene[311]),
based nonlinear optics is in its initial stage and deserves further cavities,[312] evanescent-mode coupling,[313] interference
attention. Till now, most reported all-optical photonic devices enhancement,[314] patterned structure.[315] 2D heterostructure-
based on 2DLMs depend on third-order nonlinear processes. based electro-optic modulators have attracted attention recently.
Zhang and co-workers[13] illustrated a high-speed, broadband, been successfully integrated into graphene-based silicon ring
waveguide-integrated electroabsorption modulator based on resonators[333] and long-range surface plasmon waveguides[334]
integrated monolayer graphene and silicon (Figure 12a). Fre- for light modulation through change in thermoinduced refractive
quencies of the incident light can be modulated over 1 GHz, index. Transparent flexible heat conductors based on gra-
with a broad operation spectrum ranging from 1.35 to 1.6 µm. phene also have been demonstrated to transfer localized heat
This integration of graphene and silicon for optical modu- in a microdisk resonator and a silicon-based Mach–Zehnder
lator may pave a new way for on-chip optical communications. interferometer.[335]
Englund and co-workers[316] demonstrated a graphene–BN
heterostructure-based electro-optic modulator integrated with a
silicon photonic crystal cavity (Figure 12b), showing operation 4.3.4. Other Modulation Approaches
frequency up to 1.2 GHz with a modulation depth of 3.2 dB.
Similarly, Lipson and co-workers[309] demonstrated a silicon- Magneto-optic modulators employing magneto-optic effects
based microring resonator (Figure 12c), providing efficient (Faraday effect or magneto-optic Kerr effect) for light modulation
light modulation with diverse advantages such as small energy obtain little attention than all-optical or electro-optic modulators
consumption, large modulation depth, and small footprint. due to the operation simplicity of all-optical and electrical strat-
Interestingly, Li and co-workers[317] illustrated a single gra- egies. Magneto-optic Faraday[336,337] and Kerr rotation[338] have
phene-based device (Figure 12d) that simultaneously provides been realized in graphene at the far-infrared,[336] terahertz,[338]
both efficient optical modulation (modulation depth of 64%) and microwave range,[337] suggesting the possibility of graphene-
and photodetection (near-infrared photodetection responsivity based magneto-optic modulators for diverse nonreciprocal
of 57 mA W−1). This novel multifunctional device may provide applications. Magnetoplasmons[339,340] and metastructures[341]
a new platform for the applications in optoelectronics. Tera- can also improve the magneto-optic response (Faraday rota-
hertz research has been one of the most investigated research tion and cyclotron resonance). There exists the other type of
fields recently, which is particularly desirable for the appli- modulators changing the refractive index of the material for
cations extending from health and environment to security. light diffraction and frequency varying by acoustic waves. These
Graphene modulators have been proposed to be suitable for acousto-optic modulators have been demonstrated in signal
working at the terahertz region[318–322] with excellent modula- modulation and pulse generation in optical telecommunica-
tion performance (>94% modulation depth[323]). Therefore, gra- tions and displays. Graphene and other 2DLMs are attracting
phene plasmonic electro-optic modulators have been proposed intensive attention for the generation, propagation, amplifica-
to be promising in the infrared and terahertz range,[324–326] tion, and detection of surface acoustic waves.[342,343] 2DLMs
due to the pristine frequency response of graphene. Particu- also have unique mechanical properties such as high Young’s
larly, 2DLMs with metamaterial structures
are attracting intensive attention for light
modulation such as polarization,[324,327]
phase,[328] amplitude,[329,330] and wavelength
modulation,[327] exhibiting exciting modu-
lation performance with broad operation
bandwidth, high modulation speed and
depth. Besides, 2D polar materials (hBN[331])
and their heterostructures (graphene–hBN
heterostructures[332]) have been proposed
to improve the light–matter interaction in
2DLMs either with surface–phonon polari-
tons, or plasmon–phonon polaritons for light
modulation.
4.3.3. Thermo-Optic Modulators
The most common type of thermo-optic

effects is based on the change in the mate-
rial refractive index with variations in tem-
perature, resulting in slow modulation speed
(approximately megahertz) due to the primi- Figure 12. a) Schematic of the graphene-based silicon waveguide modulator. Reproduced
tively slow thermal diffusivity. Thus, thermo- with permission.[13] Copyright 2011, Nature Publishing Group. b) Schematic of a graphene–
optic modulators are usually employed for hBN heterostructure-based planar photonic crystal (PPC) cavity modulator. Reproduced with
permission.[316] Copyright 2015, American Chemical Society. c) Schematic of a graphene-based
applications in optical routing and switching,
silicon nitride ring resonator modulator. Reproduced with permission.[309] Copyright 2015,
where high speed is not indispensable. Nature Publishing Group. d) Schematic illustration of the dual layer graphene modulator/
Because of the highly intrinsic thermal con- detector integrated on a planarized waveguide. Reproduced with permission.[317] Copyright
ductivity, graphene-based electric heaters have 2014, American Chemical Society.
modulus combined with a low loss, indicating promising appli- of 2D vdWHs have also exhibited much significances in the
cations for mechano-optic modulators. For instance, graphene recent years such as the interaction at the interface, which may
can be actuated up to high mechanical vibration frequencies provide a new degree of freedom for modulating the interaction
(more than few hundred megahertz), which may be desirable in 2D vdWHs.[187,347] The controllable preparation of large-scale
for modulation of microwave photons.[344] These novel types of 2D vdWHs is also indispensable for the industrial integra-
optical modulators provide more possibilities for applications tion. The main obstacle to obtain large-scale 2D vdWHs is the
in various fields and still need more attention. well-controlled crystallinity, uniformity, and thickness. Gener-
ally, direct growth via vapor deposition is one of the most used
methods.[348] The other way is chalcogenization of the metal
5. Conclusions and Outlook precursors predeposited on the substrate.[349] In order to obtain
more uniform large-scale 2DLMs, there are some reports on
2DLM-based vdWHs have a booming development in recent chalcogenization of the metal precursors with the substrates
years. In this feature article, we have comprehensively pre- pretreated by some organics, which can adsorb metal precur-
sented the preparation methods, energy band alignments, and sors and disperse them uniformly.[350]
applications in optoelectronics in three primary aspects: light-
emitting diodes (such as single defect light-emitting diodes,
circularly polarized light emission arising from valley polari- 5.1. Outlook for LEDs
zation), photodetectors (such as photo-thermionic, tunneling,
electrolyte-gated, and broadband photodetectors), and optical Monolayer TMD semiconductors with direct bandgaps of vis-
modulators (such as graphene integrated with silicon tech- ible to near-infrared ranges have demonstrated promising
nology, and graphene/hBN heterostructure). These reports on applications in LEDs. Compared with lateral p–n junction with
2D vdWHs suggest significant applications in the next-genera- the active area localized by the depletion region, vertical hetero-
tion optoelectronics. However, the family of 2D vdWHs is still structure based on monolayer TMDs may be more efficient for
developing, both in terms of variety of materials and construc- carrier injection due to the large active region at the whole over-
tion of devices, and it seems like just beginning. There are still lapping region. However, the EL performance is drastically lim-
so many kinds of 2D materials unknown, which may impede ited by the leakage current at the interface of vertically stacked
the diversity and multifunctionality of 2D vdWHs. Although p–n junctions. Thus, there are some directions to improve the
mechanical transfer is beneficial for investigating the physical performance of LEDs:
properties of 2D vdWHs, it is difficult for integration with the
industrial semiconductor technology due to the uncontrollable (a) The leakage current can be efficiently weakened by
size and thickness. Although some reports on the synthesizing inserting tunneling layers such as hBN into the p–n
2D vdWHs by CVD methods,[63,65,73,85] it is still a great challenge junction, resulting in long lifetime of excitons in
to controlled-synthesize more novel 2D vdWHs based on a the vertically p–n junction. Thus, the EL quantum
variety of 2D materials by CVD methods, which is a promising efficiency can be improved by this strategy for verti-
route for large-area and high-quality 2D vdWHs and is prospec- cally p–n junction.[74] The tunneling layer can also be
tive for compatibility with industrial optoelectronics. Recently, extended to other insulators such as Al2O3 and Ta2O5,
2D nonlayered materials have attracted significant attention due resulting in different tunneling barriers, which may
to possessing both novel properties of their bulk counterparts induce more light emission properties;
and unique characteristics induced by the 2D morphology.[345] (b) Using graphene as contacting electrodes can also help
For example, the surfaces of 2D nonlayered materials are to promote efficient injection of both holes and elec-
filled with dangling bonds, which do not exist in layered mate- trons in the whole junction region;
rials, modulating the charge transfer which may induce novel (c) Monolayer TMD-based LEDs usually show low efficient
transfer characteristic in electronics and optoelectronics. How- carrier injection. An alternative way to possess both the
ever, it is much difficult to realize the controllable synthesis of direct bandgap and high efficient carrier injection is to
2D nonlayered materials due to the intrinsic isotropic chemi- employ the multilayer direct bandgap 2DLMs such as
cally bonded nature, not to mention the 2D nonlayered mate- GaTe and In2Se3;[351,352]
rial-based heterostructures. CVD growth is still an efficient way (d) The white LED also needs more attention due to the
to realize the controllable synthesis of 2D nonlayered material- significant potential in lighting and display applica-
based heterostructures if the controllability of kinetics can be tions, which can be realized by multilayer-stacked
introduced to stimulate the 2D anisotropic growth. Besides, TMDs with colorful emission spectra;
the lateral vdWHs have been reported rarely due to the diffi- (e) Thermal-induced light emission can improve the
culty to obtain sharp and clean interfaces.[63] Unknown physics brightness of the 2DLM-based LEDs. Thus, it may have
from different vdWHs such as the band alignments, built-in exciting effects in vdWH-based LEDs.
electric field, charge transfer, and surface reconstruction need
to be further probed.[59] Although most physics of 2D mate- Apart from the common LEDs based on p–n junctions
rials show strong relations with the layers such as the energy emitted by recombination of injected electrons and holes, LEDs
band structures, the layer-dependent physical properties of with new mechanisms and applications are also very impor-
2D vdWHs still need significant attention, which may generate tant. For example, the electrically tunable and circularly valley-
new functionalities.[346] Notably, the angle-dependent physics LED was realized in p+-Si/WS2/n-Indium tin oxide (ITO)-based
heterojunction, which opens up new opportunities for the bandgap limitations, and so forth, which have exhibited
emerging valley-based optoelectronics. Single photons can be excellent results in photodetectors based on individual
generated by quantum emitters (from quantum confined struc- 2DLMs. Thus, it is anticipated that these localized
tures such as defects), which is much significant for the applica- fields will significantly affect the photodetection of
tions in high-resolution metrology and quantum information. 2D vdWHs. The influence mechanisms of these local-
For example, single photon emitter based on graphene/hBN/ ized fields may be different from those on individual
WSe2/hBN/graphene has been fabricated with a very sharp 2DLMs, which also need more attention;
photon emission spectrum, which provides a new platform for (c)
In order to improve the absorption efficient, some
applications of LEDs. Furthermore, laser (coherent light source) optical approaches such as plasmonic technologies,
has been realized in the 2D system.[225] However, the reports on optical waveguides, and microcavities, are very useful,
laser generated by 2D vdWHs are rare, which still needs sig- resulting in the increasing of sensitivity;
nificant attempts. Besides, scalable fabrication of 2D vdWHs (d)
These strategies mentioned above can also be inte-
will be the first obstacle for the industrial integration. As dis- grated into the device, which may lead to a further
cussed above, CVD growth is more promising than mechanical improvement of the photodetection performance.
transfer. However, it is very difficult to control the physical prop-
erties at the interface especially for the increasing layers such as As the same with LEDs, the practical applications of het-
the atomic dispersing at the interfaces. Thus, the controllable erostructures based on 2D vdWHs are also blocked by con-
preparation of 2D vdWHs still remains a great challenge. Fur- trollably large-scale preparation. Furthermore, the flexible
thermore, flexible LEDs are also attractive for many applications photodetectors based on 2D vdWHs could be applied to
in wearable optoelectronics, while the flexible LEDs based on many applications such as military communications, remote
2D vdWHs are rarely reported. sensing, biological imaging, and so forth, which are also
worth attention.
5.2. Outlook for Photodetectors

5.3. Outlook for Optical Modulators
Various kinds of photodetectors based on 2D vdWHs, including
photovoltaic, photo-thermionic, tunneling, electrolyte-gated, So far, the 2D vdWH-based optical modulators have shown
and broadband photodetectors, have been reported in recent great opportunities for optical modulation. However, the past
years and have demonstrated great promising applications in and current reports are mostly focused on graphene and con-
optoelectronics. However, there are many challenges left in this ceptual devices. Now, from the scientific and technological
field. In order to fabricate high-performance photodetectors, viewpoints, manipulation of the vdWHs to precisely tailor the
reasonable device designs and suitable materials for different performance requirements of the optical modulators still faces
parts of photodetectors are required. The most common photo major urgent challenges:
detectors based on 2D vdWHs are p–n diodes, which usually
possess fast response. However, those p–n diodes show low (a) There is plenty of room for optical modulators based on
responsivities due to the low carrier concentration. Photode- 2D vdWHs with materials other than graphene, such
tectors based on 2D vdWHs dominated by tunneling current as TMDs, black phosphorous with their unique band
is coming into view recently due to the significant promising structures and spectral responses;
applications in low power consumption optoelectronics. How- (b) As mentioned above, heterostructures with controllable
ever, tunneling current is susceptible to the quality of the inter- interlayer distance, twist angles, and different thick-
face, leading it to be uncontrollable. Thus, the controllable nesses may offer new degrees of freedom for optical
preparation of the interface is very important. Besides, the layer modulation. Multifunctional optical modulators (such
number-dependent band alignments will significantly affect the as a multifunctional modulator and photodetector) have
photodetection of 2D vdWHs. So far, most reported 2D vdWH- been demonstrated with 2D materials;
based photodetectors are composed of each of the layered mate- (c) Moreover, heterostructure-based optical modulators
rials, which show limited improvement of the photodetection may demonstrate diverse multifunctions;
performance. There are some directions that can improve the (d) Many strategies such as ion gel gating increasing car-
photodetection performance further: rier density and nanoplasmonics for faster response
and smaller footprint;
(a) Novel approaches for chemical doping and surface (e) It is also important to exploring new mechanisms and
treatment of the heterojunction should be researched, configurations for heterostructure-based optical modu-
which is a viable way to improve or modulate photode- lation such as magnetically or mechanically induced
tection performance; effects, which may provide new degree of freedoms to
(b) Introducing localized fields may also affect the junction realize the multifunctional modulators.
such as ferroelectric field, floating gate field, tempera-
ture gradient field, and so on, which can either reduce In summary, the recent booming developments on the explo-
the dark current or improve the photogain. These ration of 2D vdWHs suggest their promising applications in the
localized fields also have other advantages such as low next-generation optoelectronics and remain grand challenges to
power consumption, wide waveband response beyond be applied in commercial applications.
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F. Montero-Silva, P. H. Rezende Goncalves, D. D. Dos Reis,
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FEATURE ARTICLE

2D Layered Material-Based van der Waals Heterostructures

applications. First, we summarize the preparation methods of

2.1. Mechanical Transfer Hua Xu received his

Table 1. Summary of typical heterostructure-based LEDs (Gr: graphene).

Table 2. Summary of typical 2D vdWH-based photodetectors (GO: graphene oxide).

Device Iph/Idark Responsivity EQE Rise time Specific detectivity References

4.3. Optical Modulators system, including polarization controllers,[272] optical limiters,[273]

4.3.3. Thermo-Optic Modulators

The most common type of thermo-optic

5.2. Outlook for Photodetectors

Acknowledgements [18] Z. Fei, T. Palomaki, S. Wu, W. Zhao, X. Cai, B. Sun,

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